Regulating local electron density by introducing single-atom is an effective strategy to improve the activity of heterogeneous photo-Fenton processes. Here N, P coordinated Fe and Ni single-atom catalysts on carbon nitrides (CN-FeNi-P) were prepared to activate H₂O₂ for contaminant mineralization under visible light irradiation. The as-prepared CN-FeNi-P presented a higher moxifloxacin degradation activity in photo-Fenton system, which was up to 3.7 times that of pristine CN, meanwhile, its TOC removal reached to 95.9 % in 60 min. Based on density functional theory calculations, the Ni single-atoms serve as the optimal reactive sites to produce •OH. The strong interaction between Fe and Ni single-atoms by P-bridging and the modulated local electron structure after introducing P into coordination environment can lower •OH formation energy. This study provides new doping strategies to design single-atom catalysts and expands the family of the Fenton-like system for advanced oxidation technologies.

通过引入单原子来调节局部电子密度是提高异质光芬顿过程活性的有效策略。在此制备了 N、P 配位的 Fe 和 Ni 在氮化碳上的单原子催化剂 (CN-FeNi-P) 以活化 H ₂ O ₂用于可见光照射下的污染物矿化。所制备的CN-FeNi-P在光-芬顿体系中表现出更高的莫西沙星降解活性，是原始CN的3.7倍，同时其TOC去除率在60 min内达到95.9%。基于密度泛函理论计算，Ni 单原子作为产生•OH 的最佳反应位点。Fe和Ni单原子之间通过P桥联的强相互作用以及将P引入配位环境后调制的局部电子结构可以降低•OH的形成能。该研究为设计单原子催化剂提供了新的掺杂策略，并扩展了用于高级氧化技术的类芬顿系统家族。